Abstract
A novel B/N co-doped porous carbon nanosheet with a high heteroatom doping content has been successfully prepared. Using amino-functionalized graphene oxide (GO) as the template, oxidation polymerization of aniline, 3-aminophenylboronic acid, and m-phenylenediamine generates GO-based polyaniline nanosheets functionalized with boronic acid (GO-CBP). After high-temperature treatment, graphene-based B/N co-doped carbon nanosheets (G-CBP) are obtained, which show a typical 2D morphology with a thickness of ∼20 nm. After CO2 activation at 1000 °C, the obtained porous carbon nanosheets (G-CBP-a) have a thickness of ∼17 nm and a high specific surface area of 363 m2 g−1. Benefiting from its high surface area, unique 2D sheet nanostructure, and high heteroatom-doping contents (5.4% B and 5.3% N), G-CBP-a exhibits excellent electrochemical performance for the oxygen reduction reaction under alkaline conditions (0.1 M KOH), with a low half-wave potential (−0.27 V for G-CBP-a versus −0.18 V for Pt/C), a dominant four-electron transfer mechanism (n = 3.78 at −0.45 V), and excellent methanol tolerance and durability (10% current decrease after 20 000 s operation), as well as a high diffusion-limiting current density (JL = −4.5 mA cm−2).
Highlights
In the belief that they are the most feasible Pt alternatives, heteroatom (N,1–5 B,6,7 S,8 P9)-doped carbon materials have attracted remarkable attention as metal-free catalysts for oxygen reduction reaction (ORR), which is the key process in fuel cells
Bene ting from the high surface area, the unique 2D sheet nanostructure, and the high heteroatom-doping contents (5.4% B and 5.3% N), G-CBPa exhibits excellent electrochemical performance with respect to the oxygen reduction reaction (ORR) under alkaline conditions (0.1 M KOH), with a low half-wave potential (À0.27 V for G-CBPa versus À0.18 V for Pt/C), a dominant four-electron transfer mechanism (n 1⁄4 3.78 at À0.45 V), and excellent methanol tolerance and durability (10% current decrease a er 20 000 s operation), as well as a high diffusion-limiting current density (JL 1⁄4 À4.5 mA cmÀ2)
The typical synthesis route towards G-CBP-a is illustrated in Scheme 1
Summary
In the belief that they are the most feasible Pt alternatives, heteroatom (N,1–5 B,6,7 S,8 P9)-doped carbon materials have attracted remarkable attention as metal-free catalysts for oxygen reduction reaction (ORR), which is the key process in fuel cells. After high-temperature treatment, graphene-based B/N co-doped carbon nanosheets (G-CBP) are obtained, which show a typical 2D morphology with a thickness of $20 nm.
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